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분자활성 촉매반응 연구단
분자활성 촉매반응 연구단
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Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts

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Title
Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts
Author(s)
Magnus H. Rønne; Dasol Cho; Monica R. Madsen; Joakim B. Jakobsen; Seunghwan Eom; Émile Escoudé; Hans Christian D. Hammershøj; Dennis U. Nielsen; Steen U. Pedersen; Mu-Hyun Baik; Troels Skrydstrup; Kim Daasbjerg
Publication Date
2020-02
Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.142, no.9, pp.4265 - 4275
Publisher
AMER CHEMICAL SOC
Abstract
© 2020 American Chemical Society.Electrocatalysis is a promising tool for utilizing carbon dioxide as a feedstock in the chemical industry. However, controlling the selectivity for different CO2 reduction products remains a major challenge. We report a series of manganese carbonyl complexes with elaborated bipyridine or phenanthroline ligands that can reduce CO2 to either formic acid, if the ligand structure contains strategically positioned tertiary amines, or CO, if the amine groups are absent in the ligand or are placed far from the metal center. The amine-modified complexes are benchmarked to be among the most active catalysts for reducing CO2 to formic acid, with a maximum turnover frequency of up to 5500 s-1 at an overpotential of 630 mV. The conversion even works at overpotentials as low as 300 mV, although through an alternative mechanism. Mechanistically, the formation of a Mn-hydride species aided by in situ protonated amine groups was determined to be a key intermediate by cyclic voltammetry, 1H NMR, DFT calculations, and infrared spectroelectrochemistry
URI
https://pr.ibs.re.kr/handle/8788114/7240
ISSN
0002-7863
Appears in Collections:
Center for Catalytic Hydrocarbon Functionalizations(분자활성 촉매반응 연구단) > Journal Papers (저널논문)
Files in This Item:
jacs.9b11806.pdfDownload

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